Electrifying Nickel‐Catalyzed Coupling of Amines to Imines Under Aqueous Conditions

ABSTRACT The selective electrocatalytic oxidation of amines to imines represents a significant advancement in organic electrochemistry, offering a green and sustainable approach to access these valuable intermediates. The development of effective and environmentally friendly synthesis techniques is highly desired because imines are used extensively in materials science, agrochemicals, and pharmaceuticals. In this study, we report the fabrication of a robust, binder‐free organic–inorganic nanohybrid electrocatalyst (Bola/Ni), constructed via electrodeposition of a boladipeptide ligand (LF‐AdiA‐FL, composed of adipic acid, L‐phenylalanine, and L‐leucine) with nickel nitrate hexahydrate on a nickel foam substrate. Detailed characterization of the nanohybrid was conducted using FE‐SEM, TEM, and XPS techniques to elucidate its surface morphology and elemental composition. The Bola/Ni catalyst demonstrates excellent activity for the oxidative coupling of amines under mild, aqueous conditions, highlighting its compatibility with a wide range of functional groups and substrates. The system achieves high product yields with minimal side reactions, demonstrating its selectivity and efficiency. Notably, the use of water as the reaction medium enhances the environmental and economic viability of the process. Furthermore, the electrocatalyst maintains its performance over seven consecutive reaction cycles, indicating its strong durability and stability. Overall, this work presents a cost‐effective, energy‐efficient, and environmentally friendly strategy for imine synthesis, contributing to the advancement of sustainable organic transformations.